US7674443B1 - Zero emission gasification, power generation, carbon oxides management and metallurgical reduction processes, apparatus, systems, and integration thereof - Google Patents
Zero emission gasification, power generation, carbon oxides management and metallurgical reduction processes, apparatus, systems, and integration thereof Download PDFInfo
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- US7674443B1 US7674443B1 US12/193,692 US19369208A US7674443B1 US 7674443 B1 US7674443 B1 US 7674443B1 US 19369208 A US19369208 A US 19369208A US 7674443 B1 US7674443 B1 US 7674443B1
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Abstract
Description
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- GAME-CHANGING TECHNOLOGIES TO STRENGTHEN THE DOMESTIC ECONOMY—to program new technologies that offer to overcome impediments to clean energy while linking extractive metallurgy to the emergent nanoscale materials sector in domestic economies, located in close physical proximity where natural resources suitable for use in the present invention are situated.
- EXPANDING DOMESTIC ENERGY OUTPUT—To create a new, inexpensive source of DOE Vision 21 compliant power and pipeline gas, to drive regional development of industry and employment; and to enable bulk hydrogen production through both a SETZE process (as defined herein) and 40% solar-cell water-splitting. Specifically, SETZE will use the new III-V photovoltaic (“PV”) cell, which can generate electricity with up to 40% efficiency, thus producing cheaper hydrogen through water splitting (“WS”) at a higher output rate, to make WS hydrogen that can be used in the recovery of elemental carbon from CO2.
- GREENHOUSE GAS MITIGATION—to achieve near zero or zero-emission power generation and CO2-free strategic metal production with a SETZE carbon oxides management subprocess (SETCOM) by converting CO2 into methane pool augmentation and elemental carbon for volume applications thereof, for example, forming carbon fiber for use in stronger/thinner precast building panels and in aircraft and automobile components.
- EXPANDING DOMESTIC MINING/MINERAL ACTIVITY—to convert undervalued natural resources containing metal-bearing minerals and exotic trace metals to nanoscale powders for use in creating highly-priced end-products (including ultrahigh performance electronic materials).
- (1) Two-Step Gasification (also referred to herein as SETGAS) for hydrogen and carbon monoxide production;
- (2) Carbon Oxides Management (also referred to herein as SETCOM); and,
- (3) Metallurgical Oxide Reduction (also referred to herein as SETMOR).
-
- After gasifier feed preparation as shown in
FIG. 1.01 and discussed above, the first of two-steps involve the simplified production of SYG through a rotary kiln gasification as exhibited inFIG. 1.02 . This method is more flexible and less-restrictive than the conventional FBR gasification alternatives; and - The second step involves the SYG separation in the gas-gas cyclonic followed by purification, into bulk hydrogen (H2) and carbon monoxide (CO) products. In a more preferred alternative embodiment, as shown in
FIG. 1.04 , the gas-gas cyclonic separator 1.04.01 of the second step takes the purified syngas 1.02.03 generated by the first step and separates it into hydrogen 1.04.02 and carbon monoxide 1.04.04 streams.
- After gasifier feed preparation as shown in
Paraffins—(2n+1)*H2 +n*CO→CnH2n+2 +n*H2O 1)
(for n=1, the first in this series is the reaction giving methane: 3*H2+CO→CH4+H2O), and
Olefins—2n*H2 +n*CO→CnH2n +n*H2O. 2)
- i) Carbon/Chlorine integrated recovery/heat exchanger system 3.05.01
CO2(g)+2*H2 WS(g)→C(s)+2*H2O(l)
CO2(g)+4*H2 WS(g)→CH4(g)+2*H2O(l)
2*HCl(g)+0.5*O2 WS(g)→Cl2(g)+H2O(l) - ii) Water splitting (WS) system 3.03.01 illustrated in
FIG. 3.03 which utilizes water from reservoir 3.02.03 (FIG. 3.02 ) and power from photovoltaic devices 3.03.04, for conventional production of secondary hydrogen H2Ws 3.03.03 and oxygen O2 WS 3.03.02, stored in unresponding storage units for subsequent use.
- iii) CO2 to methane synthesis 3.05.02 to pipeline gas 1.03.02 and petrochemicals 1.03.01. The application of the second reaction under (i), a Lurgi gasification reaction, is applied here and then integrated into SETCOM.
- iv) CO2 to urea synthesis 3.05.03 then to petrochemicals' intermediates 1.03.03 input for plastics and resin products and 1.06.10 urea input for fertilizer and livestock feed production.
- v) CO2 to elemental carbon then to carbon-fiber, carbon-fiber reinforced plastic (CFRP) and other composites. The first reaction under (i) produces elemental carbon from the hydrogenation of CO2 with the lower-cost hydrogen (WS). In the SETCOM method for producing carbon fibers (CF), the elemental carbon from 3.05.01 will be used in thermally-assisted impregnation 3.05.06 of precursor rayon—a polymer with only 44.5% wt. initial carbon content, to achieve a greater nominal carbon content greater than about 82%, preferably from 82 to 88% (polyacrylonitrile (PAN)— a precursor with 85% wt. initial carbon, is traditionally preferred but costly). From the enhanced rayon precursor, intermediate carbon filament is made by oxidation and thermal pyrolysis. As with all polymers, the precursor molecules are long chains, that are aligned in the process of drawing fibers. These fibers bond side-to-side when heated, forming narrow sheets that eventually merge to form a single, jelly roll-shaped material with 92-96% by weight carbon content. The carbon fibers are further enhanced as high modulus or high strength material through additional heat treatment steps. Regarding the economics of CF applications, while PAN-based CF is seen as ideal for aircraft materials, high-end passenger vehicles and other high-tech applications, it's too costly for other potentially major applications such as CF-reinforced precast structural panels that are poised to drive far reaching changes in building design and construction. The potentially lower-cost process path afforded by SETZE rayon CF, may reduce product cost to a range that makes CF an economic surrogate for steel rebar and welded-mesh in the current precast structural materials sector.
Al2O3.3H2O (gibbsite)+2OH−(aq)→2Al(OH)(aq)
⋄H=+20.9 kJ/mol Al
2. Precipitation
2Al(OH)(aq))→Al2O3.3H2O(gibbsite)+2OH−(aq)
⋄H=−20.9 kJ/mol Al
3. Calcination of Hydrate Giving Alumina
Al2O3.3H2O(gibbsite))→Al2O3(s,⋄)+3H2O (l)
⋄H=+26.8 kJ/mol Al
4. Electrolysis of Alumina Giving Aluminum Metal
Al2O3(s,⋄)+1.5C(s)→2 Al (s)+1.5 CO2(g)
⋄H=+542.7 kJ/mol Al
Total: BHH Process' net standard enthalpy change=+569.5 kJ/mol Al.
Setze Reduction Process
1. Chlorination
⋄H=−105.2 kJ/mol Al
2. SETZE Chloride Reduction
⋄H=+371.0 kJ/mol Al
3. Chlorine Recovery
⋄H=−151.5 kJ/mol Al
Subtotal (BHH-comparable): SETZE Process' net standard enthalpy change=+114.3 kJ/mol Al.
4. Carbon Recovery
⋄H=+133.6 kJ/mol Al
5. Ceramic Synthesis
⋄H=−190.0 kJ/mol Al
Total: SETZE Process' net standard enthalpy change=+57.9 kJ/mol Al.
- i) Rotary kiln carbochlorination of metal oxides with CO as reactant (discussed above with respect to
FIG. 2.02 ) rather than coke.
Al2O3+3*Cl2+3*CO→2*AlCl3+3*CO2
Cr2O3+3*Cl2+3*CO→2*CrCl3+3*CO2
Fe2O3+3Cl2+3*CO→2*FeCl3+3*CO2
Ga2O3+3*Cl2+3*CO→2*GaCl3+3*CO2
In2O3+3*Cl2+3*CO→2*InCl3+3*CO2
Sc2O3+3*Cl2+3*CO→2*ScCl3+3*CO2
SiO2+2*Cl2+2*CO→SiCl4+2*CO2
TiO2+2*Cl2+2*CO→TiCl4+2*CO2
V2O5+4*Cl2+5*CO→2*VCl4+5*CO2
ZrO2+2*Cl2+2*CO→ZrCl4+2*CO2
- ii) Capture of CO2 2.02.03 from carbochlorination as input to SETCOM's integrated recovery/heat exchanger subsystem (bullet i, page 30).
- iii) The SETMOR MFBR 2.02.02 separates and purifies the metchlors for input to Plasma Gas Reduction (PGR) reactor 2.03.01 or Plasma Oxides Synthesis (POS) reactor 2.04.01.
- iv) Referring to
FIG. 2.03 , SETZE Plasma Gas Reduction 2.03.01 of metchlors 2.02.04, to nanoscale-range or dendritically-shaped metal powders utilizes a plasma gas reduction (PGR) reactor 2.03.01 that receives metchlors 2.02.04, power 3.04.03, preferably from HCC powerplant, and H2 SYG 1.04.02. Reactor 2.03.01 produces HCl 2.03.02 and metal powders that are degassed and cooled in facility 2.03.03 and refined in metal powders refinery 2.03.04 to produce elemental metal powders that are stored in segregated silos 2.03.05. The HCl gas is sent to the chlorine recovery 3.06.03. It should be understood that reactor 2.03.01, degassing and cooling facility 2.03.03 and refinery 2.03.04 actually represent a plurality of lines of reactors, facilities and refineries, each of which is dedicated to the reduction of a specific metchlor, such that the specific metchlor is cooled, degassed, and refined, and then stored separately. Only a single reactor and subsequent processing facilities are shown to simplify the discussion. A suitable technique may be employed based broadly on known technology advanced by the U.S. Naval Research Labs and Idaho National Engineering Labs (INEL), which sought a cheaper method for producing titanium metal that was more direct (less complex) and less expensive than the traditional Kroll process: (TiO2+2*Cl2+C→TiCl4+CO2/2*Mg+TiCl4→2*MgCl2+Ti). The Kroll process uses coke (rather than CO) as an oxygen sink in the first reaction, and expensive magnesium is consumed in the second reaction. It also requires two days to process a batch yielding only a few tons high-purity titanium per process path/reactor.
AlCl3+1.5*H2→Al+3*HCl
CrCl3+1.5*H2→Cr+3*HCl
FeCl3+1.5*H2→Fe+3*HCl
GaCl31.5*H2→Ga+3*HCl
InCl3+1.5*H2→In+3*HCl
ScCl3+1.5*H2→Sc+3*HCl
SiCl4+2*H2→Si+4*HCl
TiCl4+2*H2→Ti+4*HCl
VCl4+2*H2→V+4*HCl
ZrCl4+2*H2→Zr+4*HCl
- v) SETZE Plasma Oxides Synthesis (POS), see
FIG. 2.04 , for oxide ceramics production utilizes a POS reactor 2.04.01 that receives metchlors 2.02.04, SynGas fuel 1.03.02 and O2 As 3.01.02 and produces chlorine gas 2.04.04 that is in turn passed to chlorine recovery 3.06.02. It also produces oxide metal powders that are provided to facility 2.04.03 for cooling and degassing, and then to refining 2.04.04 to produce ceramic powders that are stored in segregated silos 2.04.05. Again, it should be understood that reactor 2.04.01 and facilities 2.04.03 and 2.04.04 are actually a plurality of reactors such that one set is dedicated to the reduction of a specific metchlor in producing a particular ceramic powder product. (A suitable procedure may be employed based broadly on DuPont Chemicals prior art in high-quality pigment production). The conversion of selected metal oxides to metchlors and back again to metal oxide ceramics yields a more perfectly formed crystalline structure for the following identified seven POS ceramic products.
Al2Cl6+1.5*O2→Al2O3+3*Cl2
2*CrCl3+1.5*O2→Cr2O3+3*Cl2
2*FeCl3+1.5*O2→Fe2O3+3Cl2
SiCl4O2→SiO2+2*Cl2
TiCl4+O2→TiO2+2*Cl2
2*VCl4+2.5*O2→V2O5+4*Cl2
2*ZrCl4+1.5*O2→Zr2O3+4*Cl2 - vi) SETZE Carbide Synthesis 3.05.07 for carbon ceramics production with powder solid-solid processing under SETMOR. Referring to
FIG. 2.05 , a process for processing the metallic powders 2.03.05 and ceramics 2.04.05 is illustrated. Various powders 2.03.05 can be selected and blended in blender 2.05.01 to produce alloy powders 2.05.02 that can be transferred to a powder feed blender line 2.05.04 and optionally mixed with ceramics from ceramic storage 2.04.05 and binder components 2.05.03 and as blended delivered for storage and/or subsequent processing by PIM line 2.06.01, rolling mill 2.07.01 or billet extrusion line 2.08.01. Or of course, the blended material could be refined and sold as a commercial product. A suitable procedure may be employed based broadly upon prior art of Randall Germann, a U.S. academic researcher in powder metallurgy. - vii) Powder Injection Molding (PIM)/sintering process (See
FIG. 2.06 ) is used to make finished products. Referring toFIG. 2.06 , a powder injection molding (PIM) process is shown. A powder feed 2.05.04, which may be a blended mixture of matter such as metals, ceramics and binders, or combinations or subcombinations thereof, and the blended mixture passed into an extruder 2.06.01. The binder is a petrochemical compound used to bind the powders in the desired form for processing. The extrudate is then passed to a debinder furnace 2.06.02, which preferably is fired by SynGas 1.03.02, in an inert furnace gas atmosphere 3.01.03, under conditions that eliminates the binder from the extrudate. The extrudate is then fed to a sintering furnace 2.06.03, which is also fired by SynGas 1.03.02 and has an inert furnace gas atmosphere 3.01.04. The sintered extrudate is then finished at station 2.06.04 and placed in inventory 2.06.05 for subsequent sale, use or distribution. - viii) Rolling and extrusion to finished powder alloy rolled products 2.07.01-02. Referring to
FIG. 2.07 , a powder rolling mill production process is shown. A powder feed 2.05.04, which may be a blended mixture of matter such as metals, ceramics and binders, or combinations or subcombinations thereof, is fed into a powder compactor and rolling mill sheeting facility 2.07.02 that will produce rolled sheet. The rolled sheet is passed to a debinder furnace 2.07.03, which preferably is fired by SynGas 1.03.02, and an inert furnace gas 3.01.03, and eliminates the binder from the sheet. The rolled metal sheet is then fed to a heat treat furnace 2.07.04, which also burns SynGas 1.03.02 and has an inert furnace gas atmosphere gas 3.01.04. After heat treatment, the sheet may be subjected to converted coil cold rolling and finishing processes in a suitable mill 2.07.05. The finished sheet, preferably in a coil, is placed in inventory 2.07.06 for subsequent sale, use or distribution. - ix) Referring to
FIG. 2.08 , a powder billet extrusion production process is shown. A powder feed 2.05.04, which may be a blended mixture of matter such as metals, ceramics and binders, or combinations or subcombinations thereof, is fed into a powder compactor 2.08.01 to form billets that are put in storage until needed. The billets, when needed, are passed to a billet reheat furnace 2.08.03, which preferably consumes SynGas 1.03.02, and an inert furnace gas 3.01.03, and when at the desired temperature are delivered to a hot extrusion process 2.08.04. The extrudate is then passed through a debinder furnace 2.08.05 and a sintering furnace 2.08.06 as the extrudate discussed above, to produce a form 2.08.07 that is put into inventory 2.06.05 for subsequent sale, use or distribution. - x) Ultrahigh performance semiconductor III-V compounds and alloy production 2.03.04, as discussed above.
SETZE Water Supply from Sea Water Desalinization
In one alternative embodiment of the invention, the SETZE facility for production of potable and process water is a thermal desalinization unit. Sea water from the nearest source point will be piped to the thermal desalinization plant sited next to the HCC power plant. The bleeding-off of superheated steam from the adjacent power plant will drive the thermal desalinization process in the separation of fresh water from brine. The gas-liquid separation of sea water is achieved at 220° F. by heat transferred from the superheated steam exhaust of the HCC unit. After separation from brine, the water vapor is cooled and condensed to purified water. The recovered brine provides a valuable input to the SETZE metallurgical subsystem, in that the chlorine needed for metallurgical reduction can be extracted from the brine.
Supplemental economic benefits from desalinization beyond fresh water. After refining, the crystallized sodium chloride (NaCl—unrefined table salt) from the brine is fed to an in-country chlor-alkali plant (nonmercury cell type) for the production of chlorine, hydrogen and caustic soda. Caustic soda will be consumed in SETZE operations or sold to pulp and paper processors or water treatment utilities). The virgin chlorine product is fed into the SETZE pool of recycled chlorine as makeup and/or sold to the external chemicals' market. Another bulk use for the recovered raw NaCl, is as input to a refinery for the production of ordinary table salt.
A residual of brine processing is the bitterns mother liquor. The rich bitterns' liquor contains halide traces such as valuable iodides, bromides, magnesium chloride, and magnesium sulfate; et al, from which marketable compounds can be extracted and sold externally. Elemental magnesium can be used as a SETZE alloying agent or sold on the chemicals and/or metals markets.
Carbochlorination of Copper
-
- Chalcopyrite Concentrate Reaction1: 5*CuFeS, +7.5*Cl2+4*CO→5*CuCl+5*FeCl2+4*CS2+2*SO2
- Chalcocite Concentrate Reaction1: 5*Cu2S+5*Cl2+2*CO→10*CuCl+2*CS2+SO2
- Bomite Concentrate Reaction1: 5*Cu5FeS4+17.5*Cl2+8*CO→25*CuCl+5*FeCl2+8*CS2+4*SO2
- Gold (native) Reaction1: Au+1.5*Cl2→AuCl3 (s) [auric chloride, a solid]
- Silver (native) Reaction1: Ag+0.5*Cl2→AgCl (s) [silver chloride, a solid]
- Chalcopyrite, Chalcocite & Bornite Reaction2: CS2+3*O2→CO2+2*SO2
- Chalcopyrite, Chalcocite & Bornite Reaction3/Plasma Gas Reduction: CuCl+0.5*H2→Cu+HCl
- Chalcopyrite and Bornite Reaction4/Plasma Gas Reduction: FeCl2+H2→Fe+2*HCl
- Gold Reaction2/Plasma Gas Reduction: AuCl3+1.5*H2→Au+3*HCl [assumes reactant auric chloride (on the left) is gaseous at higher process heat of the PGR reactor]
- Silver Reaction2/Plasma Gas Reduction: AgCl+0.5*H2→Ag+HCl [assumes reactant silver chloride (on the left) is gaseous at higher process heat of the PGR reactor]
As one will understand, the reactions are stoichiometric, and the relationship of the copper compounds on either side involve only Cu-I—in accordance with “ . . . all the known copper sulfides should be considered as purely monovalent copper compounds . . . ” in the URL: http://en.wikipedia.org/wiki/Copper(II)_sulfide. Additionally, there are three oxidation levels for copper, Cu-I, Cu-II and rarely Cu-III.
Claims (29)
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